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The presence of inclusions, twinning, and low-angle grain boundaries, demanded to exist by the third law of thermodynamics, drive the behavior of quantum materials. Identification and quantification of these structural complexities often requires destructive techniques. X-ray micro-computed tomography (µCT) uses high-energy X-rays to non-destructively generate 3D representations of a material with micron/nanometer precision, taking advantage of various contrast mechanisms to enable the quantification of the types and number of inhomogeneities. We present case studies of µCT informing materials design of electronic and quantum materials, and the benefits to characterizing inclusions, twinning, and low-angle grain boundaries as well as optimizing crystal growth processes. We discuss recent improvements in µCT instrumentation that enable elemental analysis and orientation to be obtained on crystalline samples. The benefits of µCT as a non-destructive tool to analyze bulk samples should encourage the community to adapt this technology into everyday use for quantum materials discovery.

 

Entropic stabilization has evolved into a strategy to create new oxide materials and realize novel functional properties engineered through the alloy composition. Achieving an atomistic understanding of these properties to enable their design, however, has been challenging due to the local compositional and structural disorder that underlies their fundamental structure-property relationships. Here, we combine high-throughput atomistic calculations and linear regression algorithms to investigate the role of local configurational and structural disorder on the thermodynamics of vacancy formation in (MgCoNiCuZn)O-based entropy-stabilized oxides (ESOs) and their influence on the electrical properties. We find that the cation-vacancy formation energies decrease with increasing local tensile strain caused by the deviation of the bond lengths in ESOs from the equilibrium bond length in the binary oxides. The oxygen-vacancy formation strongly depends on structural distortions associated with the local configuration of chemical species. Vacancies in ESOs exhibit deep thermodynamic transition levels that inhibit electrical conduction. By applying the charge-neutrality condition, we determine that the equilibrium concentrations of both oxygen and cation vacancies increase with increasing Cu mole fraction. Our results demonstrate that tuning the local chemistry and associated structural distortions by varying alloy composition acts an engineering principle that enables controlled defect formation in multi-component alloys.

 

Rutile compounds have exotic functional properties that can be applied for various electronic applications; however, the limited availability of epitaxial substrates has restricted the study of rutile thin films to a limited range of lattice parameters. Here, rutile GeO 2 is demonstrated as a new rutile substrate with lattice parameters of [Formula: see text] and [Formula: see text]. Rutile GeO 2 single crystals up to 4 mm in size are grown by the flux method. X-ray diffraction reveals high crystallinity with a rocking curve having a full width half-maximum of 0.0572°. After mechanical polishing, a surface roughness of less than 0.1 nm was obtained, and reflection high-energy electron diffraction shows a crystalline surface. Finally, epitaxial growth of (110)-oriented TiO 2 thin films on GeO 2 substrates was demonstrated using molecular beam epitaxy. Templated by rutile GeO 2 substrates, our findings open the possibility of stabilizing new rutile thin films and strain states for the tuning of physical properties. 

BAs is a III–V semiconductor with ultra-high thermal conductivity, but many of its electronic properties are unknown. This work applies predictive atomistic calculations to investigate the properties of BAs heterostructures, such as strain effects on band alignments and carrier mobility, considering BAs as both a thin film and a substrate for lattice-matched materials. The results show that isotropic biaxial in-plane strain decreases the band gap independent of sign or direction. In addition, 1% biaxial tensile strain increases the in-plane electron and hole mobilities at 300 K by >60% compared to the unstrained values due to a reduction of the electron effective mass and of hole interband scattering. Moreover, BAs is shown to be nearly lattice-matched with InGaN and ZnSnN₂, two important optoelectronic semiconductors with tunable band gaps by alloying and cation disorder, respectively. The results predict type-II band alignments and determine the absolute band offsets of these two materials with BAs. The combination of the ultra-high thermal conductivity and intrinsic p-type character of BAs, with its high electron and hole mobilities that can be further increased by tensile strain, as well as the lattice-match and the type-II band alignment with intrinsically n-type InGaN and ZnSnN₂demonstrate the potential of BAs heterostructures for electronic and optoelectronic devices.

 

Memristors have emerged as transformative devices to enable neuromorphic and in‐memory computing, where success requires the identification and development of materials that can overcome challenges in retention and device variability. Here, high‐entropy oxide composed of Zr, Hf, Nb, Ta, Mo, and W oxides is first demonstrated as a switching material for valence change memory. This multielement oxide material provides uniform distribution and higher concentration of oxygen vacancies, limiting the stochastic behavior in resistive switching. (Zr, Hf, Nb, Ta, Mo, W) high‐entropy‐oxide‐based memristors manifest the “cocktail effect,” exhibiting comparable retention with HfO₂‐ or Ta₂O₅‐based memristors while also demonstrating the gradual conductance modulation observed in WO₃‐based memristors. The electrical characterization of these high‐entropy‐oxide‐based memristors demonstrates forming‐free operation, low device and cycle variability, gradual conductance modulation, 6‐bit operation, and long retention which are promising for neuromorphic applications.